All existing solar cell materials including hybrid perovskites show rather small absorption coefficient (α) of ≈104 cm−1 in the bandgap (Eg) transition region. The weak band‐edge light absorption is an essential problem, limiting conversion efficiency particularly in a tandem solar cell. Herein, all distorted chalcogenide perovskites (BaZrS3, SrZrS3, BaHfS3, and SrHfS3) are found experimentally to exhibit extraordinary high α exceeding 105 cm−1 near Eg, indicating the highest band‐edge α among all known solar cell materials. The giant absorption in the Eg region, which is consistent with the first principles, arises from the intense p–d interband transition enabled by dense S 3p valence states. For solar cell application, low‐gap BaZrS3 derivatives, Ba(Zr,Ti)S3 and BaZr(S,Se)3, are further synthesized. Among the possible candidates of top‐cell materials, an earth‐abundant and nontoxic Ba(Zr,Ti)S3 alloy shows great potential, reaching a maximum potential efficiency exceeding 38% in a chalcogenide perovskite/crystalline Si tandem architecture.

Inspired by the successful synthesis of alkaline-earth-metals-based electrides [CaAlO](e) (C12A7:e) and [CaN]:e and high-throughput database screening results, we explore the potential for new electrides to emerge in the Sr-P system through a research approach combining ab initio evolutionary structure searches and experimental validation. Through employing an extensive evolutionary structure search and first-principles calculations, we first predict the new structures of a series of strontium phosphides: SrP, SrP, SrP and SrP. Of these structures, we identify SrP and SrP as being potential electrides with quasi-one-dimensional (1D) and zero-dimensional (0D) character, respectively. Following these theoretical results, we present the successful synthesis of the new compound SrP and the experimental confirmation of its structure. Although density functional calculations with the generalized gradient approximation predict SrP to be a metal, electrical conductivity measurement reveal semiconducting properties characterized by a distinct band gap, which indicates that the newly synthesized SrP is an ideal one-dimensional electride with the half-filled band by unpaired electrons. In addition to presenting the novel electride SrP, we discuss the implications of its semiconducting nature for 1D electrides in general and propose a mechanism for the formation of electrides with an orbital level diagram based on first-principles calculations.

It is thought that strong electron correlation in an insulating parent phase would enhance a critical temperature (Tc) of superconductivity in a doped phase via enhancement of the binding energy of a Cooper pair as known in high-Tc cuprates. To induce a superconductor transition in an insulating phase, injection of a high density of carriers is needed (e.g., by impurity doping). An electric double-layer transistor (EDLT) with an ionic liquid gate insulator enables such a field-induced transition to be investigated and is expected to result in a high Tc because it is free from deterioration in structure and carrier transport that are in general caused by conventional carrier doping (e.g., chemical substitution). Here, for insulating epitaxial thin films (∼10 nm thick) of FeSe, we report a high Tc of 35 K, which is 4× higher than that of bulk FeSe, using an EDLT under application of a gate bias of +5.5 V. Hall effect measurements under the gate bias suggest that highly accumulated electron carrier in the channel, whose area density is estimated to be 1.4 × 1015 cm–2 (the average volume density of 1.7 × 1021 cm–3), is the origin of the high-Tc superconductivity. This result demonstrates that EDLTs are useful tools to explore the ultimate Tc for insulating parent materials.

A current issue facing light-emitting devices is a missing suitable material for green emission. To overcome this, we explore semiconductors possessing (i) a deep conduction band minimum (CBM) and a shallow valence band maximum (VBM), (ii) good controllability of electronic conductivity and carrier polarity, and (iii) a directly allowed band gap corresponding to green emission. We focus on early transition metal (eTM)-based perovskites. The eTM cation’s high and stable valence state makes its carrier controllability easy, and the eTM’s nonbonding d orbital and the anion’s p orbital, which constitute the deep CBM and shallow VBM, are favorable to n- and p-type doping, respectively. To obtain a direct band gap, we applied a scheme that folds the bands constituting the VBM at the zone boundary to the zone center where the CBM appears. Orthorhombic SrHfS3 was chosen as the candidate. The electrical conductivity was tuned from 6 × 10–7 to 7 × 10–1 S·cm–1 with lanthanum (La) doping and to 2 × 10–4 S·cm–1 with phosphorus (P) doping. Simultaneously, the major carrier polarity was controlled to n type by La doping and to p type by P doping. Both the undoped and doped SrHfS3 exhibited intense green photoluminescence (PL) at 2.37 eV. From the PL blue shift and short lifetime, we attributed the emission to a band-to-band transition and/or exciton. These results demonstrate that SrHfS3 is a promising green-light-emitting semiconductor.

High-critical-temperature (T c ) superconductivity at 48 K is reported for hydrogen-doped SmFeAsO epitaxial films on MgO single-crystal substrates. The key processes are pulsed laser deposition to grow undoped SmFeAsO epitaxial films and subsequent topotactic chemical reaction using CaH 2 powders under evacuated silica-glass ampule atmosphere. Based on this post-deposition thermal annealing treatment that we have developed, a maximum hydrogen concentration x = ~0.35 was realized in SmFeAs(O 1x H x ). Disordered hydrogen-substitution at O sites is experimentally confirmed directly by atomic-scale microstructural observations. Magnetization measurement validates the bulk nature of the high-T c superconductivity in the films. This method will become an effective and general method to fabricate various high-quality oxyhydride epitaxial films.